65 research outputs found
Chemical, Structural, and Morphological Changes of a MoVTeNb Catalyst during Oxidative Dehydrogenation of Ethane
MoVTeNb mixed oxide, a highly active and
selective catalyst for the oxidative dehydrogenation of ethane to
produce ethylene, exhibits the so-called M1 and M2 crystalline
phases. The thermal stability of the MoVTeNb catalytic system
was assessed under varying reaction conditions; to this end, the
catalyst was exposed to several reaction temperatures spanning
from 440 to 550 °C. Both the pristine and spent materials were
analyzed by several characterization techniques. The catalyst
was stable below 500 °C; a reaction temperature of â„500 °C
brings about the removal of tellurium from the intercalated
framework channels of the M1 crystalline phase. Rietveld
refinement of X-ray diffraction patterns and microscopy results showed that the tellurium loss causes the progressive partial
destruction of the M1 phase, thus decreasing the number of active sites and forming a MoO2 crystalline phase, which is inactive
for this reaction. Raman spectroscopy confirmed the MoO2 phase development as a function of reaction temperature. From highresolution
transmission electron microscopy and energy-dispersive X-ray spectroscopy analyses it was noticed that tellurium
departure occurs preferentially from the end sides of the needlelike M1 crystals, across the [001] plane. Detailed analysis of a
solid deposited at the reactor outlet showrf that it consisted mainly of metallic tellurium, suggesting that the tellurium
detachment occurs via reduction of Te4+ to Te0 due to a combination of reaction temperature and feed composition. Thus, in
order to sustain the catalytic performance exhibited by MoVTeNb mixed oxide, hot spots along the reactor bed should be
avoided or controlled, maintaining the catalytic bed temperature below 500 °C.This work was financially supported by the Instituto Mexicano del Petroleo.Valente, JS.; Armendariz-Herrera, H.; Quintana-Solorzano, R.; Del Angel, P.; Nava, N.; Masso RamĂrez, A.; LĂłpez Nieto, JM. (2014). Chemical, Structural, and Morphological Changes of a MoVTeNb Catalyst during Oxidative Dehydrogenation of Ethane. ACS Catalysis. 4:1292-1301. doi:10.1021/cs500143jS12921301
Genetic determinants of co-accessible chromatin regions in activated T cells across humans.
Over 90% of genetic variants associated with complex human traits map to non-coding regions, but little is understood about how they modulate gene regulation in health and disease. One possible mechanism is that genetic variants affect the activity of one or more cis-regulatory elements leading to gene expression variation in specific cell types. To identify such cases, we analyzed ATAC-seq and RNA-seq profiles from stimulated primary CD4+ T cells in up to 105 healthy donors. We found that regions of accessible chromatin (ATAC-peaks) are co-accessible at kilobase and megabase resolution, consistent with the three-dimensional chromatin organization measured by in situ Hi-C in T cells. Fifteen percent of genetic variants located within ATAC-peaks affected the accessibility of the corresponding peak (local-ATAC-QTLs). Local-ATAC-QTLs have the largest effects on co-accessible peaks, are associated with gene expression and are enriched for autoimmune disease variants. Our results provide insights into how natural genetic variants modulate cis-regulatory elements, in isolation or in concert, to influence gene expression
Deficient histone H3 propionylation by BRPF1-KAT6 complexes in neurodevelopmental disorders and cancer
Lysine acetyltransferase 6A (KAT6A) and its paralog KAT6B form stoichiometric complexes with bromodomain- and PHD finger-containing protein 1 (BRPF1) for acetylation of histone H3 at lysine 23 (H3K23). We report that these complexes also catalyze H3K23 propionylati
Stretch-activated ion channel TMEM63B associates with developmental and epileptic encephalopathies and progressive neurodegeneration
By converting physical forces into electrical signals or triggering intracellular cascades, stretch-activated ion channels allow the cell to respond to osmotic and mechanical stress. Knowledge of the pathophysiological mechanisms underlying associations of stretch-activated ion channels with human disease is limited. Here, we describe 17 unrelated individuals with severe early-onset developmental and epileptic encephalopathy (DEE), intellectual disability, and severe motor and cortical visual impairment associated with progressive neurodegenerative brain changes carrying ten distinct heterozygous variants of TMEM63B, encoding for a highly conserved stretch-activated ion channel. The variants occurred de novo in 16/17 individuals for whom parental DNA was available and either missense, including the recurrent p.Val44Met in 7/17 individuals, or in-frame, all affecting conserved residues located in transmembrane regions of the protein. In 12 individuals, hematological abnormalities co-occurred, such as macrocytosis and hemolysis, requiring blood transfusions in some. We modeled six variants (p.Val44Met, p.Arg433His, p.Thr481Asn, p.Gly580Ser, p.Arg660Thr, and p.Phe697Leu), each affecting a distinct transmembrane domain of the channel, in transfected Neuro2a cells and demonstrated inward leak cation currents across the mutated channel even in isotonic conditions, while the response to hypo-osmotic challenge was impaired, as were the Ca2+ transients generated under hypo-osmotic stimulation. Ectopic expression of the p.Val44Met and p.Gly580Cys variants in Drosophila resulted in early death. TMEM63B-associated DEE represents a recognizable clinicopathological entity in which altered cation conductivity results in a severe neurological phenotype with progressive brain damage and early-onset epilepsy associated with hematological abnormalities in most individuals. Genetics of disease, diagnosis and treatmen
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Toward a next generation particle precipitation model: Mesoscale prediction through machine learning (a case study and framework for progress)
We advance the modeling capability of electron particle precipitation from the magnetosphere to the ionosphere through a new database and use of machine learning tools to gain utility from those data. We have compiled, curated, analyzed, and made available a new and more capable database of particle precipitation data that includes 51 satellite years of Defense Meteorological Satellite Program (DMSP) observations temporally aligned with solar wind and geomagnetic activity data. The new total electron energy flux particle precipitation nowcast model, a neural network called PrecipNet, takes advantage of increased expressive power afforded by machine learning approaches to appropriately utilize diverse information from the solar wind and geomagnetic activity and, importantly, their time histories. With a more capable representation of the organizing parameters and the target electron energy flux observations, PrecipNet achieves a 50\% reduction in errors from a current state-of-the-art model (OVATION Prime), better captures the dynamic changes of the auroral flux, and provides evidence that it can capably reconstruct mesoscale phenomena. We create and apply a new framework for space weather model evaluation that culminates previous guidance from across the solar-terrestrial research community. The research approach and results are representative of the `new frontier' of space weather research at the intersection of traditional and data science-driven discovery and provides a foundation for future efforts
Thermodynamic Properties of Nonstoichiometric Nickel Tellurides and of Tellurium
As part of a thermodynamic study of NiTe and NiTe/sub 2/, an attempt was made to gather data which would determine zero-point entropies as a function of composition. Part of the necessary data have been gathered, and in addition a number of other pertinent or interesting properties of the nickel tellurides, and of Te, have been investigated. Specific heats from 4 to 350 deg K have been measured on NiTe/sub 1.1/ NiTe/sub 1.5/, and NiTe/sub 2.0/, and the thermodynamic functions of these and all intermediate compositions may be considered accurately known over this temperature range. The method employed was conventional precise adiabatic calorimetry in an existing apparatus. The melting point of Te has been redetermined and the highly discordant literature critically reexamined; the triple point may now be stated with some confidence to be 449.7 plus or minus 0.2 deg C. The dissociation pressures of compositions from NiTe/sub 1.5/ to NiTe/ sub 2.0/ have been accurately measured at temperatures up to 780 deg C in order to determine the partial molal free energies and entropies of Te in these compounds. These measurements have incidentally elucidated the phase behavior in the Te-rich region, showing a high solubility of Ni in liquid Te at elevated temperatures, and incongruent melting of the solid solutions such that Te-rich solid solutions are unstable at elevated temperatures. By extrapolation, the boiling point of Te is computed to be 993.6 plus or minus 2 deg C. and the heat of vaporization to be 33,850-908 t cal/mole (one mole equals two gram-atoms). with an accuracy of plus or minus several hundred calories, from the triple point to t = 850 deg , or perhaps 950 deg C. This figure may be considered more accurate, though stated with less precision, than those of previous investigators. (auth
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